Abstract [en]

Biosensors are devices that detect biological elements and then transmit a readable signal. Biosensors can automatize diagnostics that would otherwise have to be performed by a physician or perhaps not be possible to perform at all. Current biosensors are however either limited to particular diseases or prohibitively expensive. In order to further the field, sensors capable of many parallel measurements at a lower cost need to be developed. Field effect transistor (FET) based sensors are possible candidates for delivering this, mainly by allowing miniaturization. Smaller sensors could be cheaper, and enable parallel measurements.

Graphene is an interesting material to use as the channel of FET-sensors. The low electrochemical reactivity of its plane makes it possible to have graphene in direct contact with the sample liquid, which enhances the signal from impedance changes. Graphene-FET based impedance sensors should be able to sense almost all possible analytes and allow for scaling without losing sensitivity.

In this work the steps needed to make graphene based biosensors are presented. An improved graphene transfer is described which by using low pressure to dry the graphene removes most contamination. A method to measure the contamination of graphene by surface enhanced Raman scattering is presented. Methods to produce double gated and electrolyte gated graphene transistors on a large scale in an entirely photolithographic process are detailed. The deposition of 1-pyrenebutyric acid (PBA) on graphene is studied. It is shown that at high surface concentrations the PBA stands up on graphene and forms a dense self-assembled monolayer. A new process of using Raman spectroscopy data to quantify adsorbents was developed in order to quantify the molecule adsorption. Biosensing has been performed in two different ways. Graphene FETs have been used to read the signal generated by a streaming potential setup. Using FETs in this context enables a more sensitive readout than what would be possible without them. Graphene FETs have been used to directly sense antibodies in high ionic strength. This sensing was done by measuring the impedance of the interface between the FET and the electrolyte.

Abstract [en]

A room-temperature polymer-assisted transfer process is developed for large-area, single-layer graphene grown by means of chemical vapor deposition (CVD). This process leads to transferred graphene layers free of polymer contamination. The absence of polymer residues boosts the surface-enhanced Raman scattering (SERS) of the CVD graphene with gold nanoparticles (Au NPs) deposited atop by evaporation. The SERS enhancement of the CVD graphene reaches similar to 120 for the characteristic 2D peak of graphene, the highest enhancement factor achieved to date, when the Au NPs are at the threshold of percolation. Our simulation supported by experiment suggests that the polymer residues persistently present on the graphene transferred by the conventional polymer-assisted method are equivalent to an ultrathin film of less than 1 nm thickness. The presence of polymer residues drastically reduces SERS due to the separation of the Au NPs from the underlying graphene. The scalability of CVD graphene opens up for the possibility of graphene-based SERS sensors.

Abstract [en]

Research on graphene field-effect transistors (GFETs) has mainly relied on devices fabricated using electron-beam lithography for pattern generation, a method that has known problems with polymer contaminants. GFETs fabricated via photo-lithography suffer even worse from other chemical contaminations, which may lead to strong unintentional doping of the graphene. In this letter, we report on a scalable fabrication process for reliable GFETs based on ordinary photo-lithography by eliminating the aforementioned issues. The key to making this GFET processing compatible with silicon technology lies in a two-in-one process where a gate dielectric is deposited by means of atomic layer deposition. During this deposition step, contaminants, likely unintentionally introduced during the graphene transfer and patterning, are effectively removed. The resulting GFETs exhibit current-voltage characteristics representative to that of intrinsic non-doped graphene. Fundamental aspects pertaining to the surface engineering employed in this work are investigated in the light of chemical analysis in combination with electrical characterization.